Aerosol Direct Radiative Forcing Research Articles

Satellite‐retrieved direct radiative forcing of aerosols over North‐East India and adjoining areas: climatology and impact assessment

ABSTRACTIn order to understand the climatic implications of atmospheric aerosols, top of atmosphere (TOA) shortwave (SW, 0.3–5 µm) fluxes and aerosol optical depth (AOD) at 550 nm retrieved simultaneously by clouds and the earth's radiant energy system (CERES) and moderate resolution imaging spectroradiometer (MODIS) instruments, respectively, are analysed over North‐East India and its adjoining areas for the period July 2002–December 2013. The aerosol‐free TOA flux obtained by establishing the linear regression between CERES SW TOA fluxes and MODIS AODs exhibits strong seasonality with peak values in monsoon and minimum in winter. Same seasonality is captured by the Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART) model, but with difference in absolute values. SBDART code is used to extend instantaneous radiative forcing estimates into 24‐h averages. AOD over the North East India region with complex terrain shows altitudinal variation with maximum value at the lowest elevation site Dhaka and minimum value at the high‐altitude locations Shillong and Aizwal. In general, strong seasonality in AOD is observed with a peak in pre‐monsoon (March–May) and dip in post‐monsoon (October–November) at all the locations. The direct instantaneous TOA shortwave aerosol radiative forcing (SWARF) shows maximum values in pre‐monsoon over all the locations except at Guwahati, Banmauk, Aizawl, and Shillong. The lowest value of instantaneous SWARF is observed in post‐monsoon except at Banmauk and Shillong. Climatologically TOA diurnally averaged SWARF varies between −6.95 W m−2 in Aizawl to −20.39 W m−2 in Shillong. In general, the TOA SW forcing efficiency is highest in monsoon at all the locations. The radiative forcing efficiency is found to be less negative when surface reflectance increases.

Aerosol direct shortwave radiative forcing effect based on SBDART model in the Pearl River Delta, Guangdong (China)

Aerosols play an important role in the energy budget of the earth-atmosphere system. In this paper, we studied aerosol shortwave direct radiative forcing (DRF) effects in Pearl River Delta based on SBDART and a 'two-layer-single-wavelength' model. Simulation results indicated that the underlying surface type and solar zenith angle have significant impacts on aerosol radiative forcing. The comparison between aerosol radiative forcing effects on urban asphalt surface and vegetation shows cooling and warming effects of aerosol shortwave radiative forcing on urban asphalt are much more apparent than that on vegetation, implying aerosols over asphalt-predominated cities will impact the local climate. Then we estimated variations of average DRF and net radiation flux with solar zenith angle in the Pearl River Delta. DRF indicates warming at solar zenith angles of 0°, 20°, 40° and 60°, but cooling at 80°. Net radiation flux increases with a decrease in aerosol optical thickness (AOT) at low elevation, but with an increase in AOT above 5 km.

Aerosol direct shortwave radiative forcing effect based on SBDART model in the Pearl River Delta, Guangdong (China)

Aerosol direct shortwave radiative forcing effect based on SBDART model in the Pearl River Delta, Guangdong (China)

Implications of RCP emissions on future PM2.5 air quality and direct radiative forcing over China

AbstractSevere PM2.5 air pollution in China and the First Grand National Standard (FGNS), implemented in 2016 (annual PM2.5 concentration target of less than 35 µg m−3), necessitate urgent reduction strategies. This study applied the nested‐grid version of the Goddard Earth Observing System (GEOS) chemical transport model (GEOS‐Chem) to quantify 2000–2050 changes in PM2.5 air quality and related direct radiative forcing (DRF) in China, based on future emission changes under the representative concentration pathway (RCP) scenarios of RCP2.6, RCP4.5, RCP6.0, and RCP8.5. In the near term (2000–2030), a projected maximum increase in PM2.5 concentrations of 10–15 µg m−3 is found over east China under RCP6.0 and RCP8.5 and less than 5 µg m−3 under RCP2.6 and RCP4.5. In the long term (2000–2050), PM2.5 pollution clearly improves, and the largest decrease in PM2.5 concentrations of 15–30 µg m−3 is over east China under all RCPs except RCP6.0. Focusing particularly on highly polluted regions, we find that Beijing‐Tianjin‐Hebei (BTH) wintertime PM2.5 concentrations meeting the FGNS occur after 2040 under RCP2.6, RCP4.5, and RCP8.5, and summertime PM2.5 concentrations reach this goal by 2030 under RCP2.6 and RCP4.5. In Sichuan Basin (SCB), wintertime PM2.5 concentrations below the FGNS occur only in 2050 under RCP2.6 and RCP4.5, although future summertime PM2.5 will be well controlled. The difficulty in controlling future PM2.5 concentrations relates to unmitigated high levels of nitrate, although NOx and SO2 emissions show substantial reductions during 2020–2040. The changes in aerosol concentrations lead to positive aerosol DRF over east China (20°–45°N, 100°–125°E) by 1.22, 1.88, and 0.66 W m−2 in 2050 relative to 2000 under RCP2.6, RCP4.5, and RCP8.5, respectively. When considering both health and climate effects of PM2.5 over China, for example, PM2.5 concentrations averaged over east China under RCP4.5 (RCP2.6) decrease by 54% (43%) in 2050 relative to 2000, but at the cost of warming with DRF of 1.88 (1.22) W m−2. Our results indicate that it will be possible to mitigate future PM2.5 pollution in China, but it will likely take two decades for polluted regions such as BTH and SCB to meet the FGNS, based on all RCP scenarios. At the same time, the consequent warming effects from reduced aerosols are also significant and inevitable.

Quantifying organic aerosol single scattering albedo over the tropical biomass burning regions

Despite growing evidence of light-absorbing organic aerosols (OAs), their contribution to the Earth's radiative budget is still poorly understood. In this study we derived a new empirical relationship that binds OA single scattering albedo (SSA), which is the ratio of light scattering to extinction, with sulfate + nitrate aerosol optical depth (AOD) and applied this method to estimate OA SSA over the tropical biomass burning regions. This method includes division of the attribution of black carbon (BC) and OA absorption aerosol optical depths from the Aerosol Robotic Network (AERONET) observation and determination of the fine-mode ratio of sea-salt and dust AODs from several atmospheric chemistry models. Our best estimate of OA SSA over the tropical biomass burning regions is 0.91 at 550 nm. Uncertainties associated with observations and models permit a value range of 0.82–0.93. Furthermore, by using the estimated OA SSA and comprehensive observations including AERONET, Moderate Resolution Imaging Spectroradiometer (MODIS) and Multi-angle Imaging Spectroradiometer (MISR), we examined the first global estimate of sulfate + nitrate AOD through a semi-observational approach. The global mean sulfate + nitrate AOD of 0.017 is in the lower range of the values obtained from 21 models participated in AeroCom phase II. The results imply that most aerosol models as well as climate models, which commonly use OA SSA of 0.96–1.0, have so far ignored light absorption by OAs and have overestimated light scattering by sulfate + nitrate aerosols. This indicates that the actual aerosol direct radiative forcing should be less negative than currently believed.

Aerosol optical, microphysical and radiative properties at regional background insular sites in the western Mediterranean

Abstract. In the framework of the ChArMEx (the Chemistry-Aerosol Mediterranean Experiment; http://charmex.lsce.ipsl.fr/) program, the seasonal variability of the aerosol optical, microphysical and radiative properties derived from AERONET (Aerosol Robotic Network; http://aeronet.gsfc.nasa.gov/) is examined in two regional background insular sites in the western Mediterranean Basin: Ersa (Corsica Island, France) and Palma de Mallorca (Mallorca Island, Spain). A third site, Alborán (Alborán Island, Spain), with only a few months of data is considered for examining possible northeast–southwest (NE–SW) gradients of the aforementioned aerosol properties. The AERONET dataset is exclusively composed of level 2.0 inversion products available during the 5-year period 2011–2015. AERONET solar radiative fluxes are compared with ground- and satellite-based flux measurements. To the best of our knowledge this is the first time that AERONET fluxes are compared with measurements at the top of the atmosphere. Strong events (with an aerosol optical depth at 440 nm greater than 0.4) of long-range transport aerosols, one of the main drivers of the observed annual cycles and NE–SW gradients, are (1) mineral dust outbreaks predominant in spring and summer in the north and in summer in the south and (2) European pollution episodes predominant in autumn. A NE–SW gradient exists in the western Mediterranean Basin for the aerosol optical depth and especially its coarse-mode fraction, which all together produces a similar gradient for the aerosol direct radiative forcing. The aerosol fine mode is rather homogeneously distributed. Absorption properties are quite variable because of the many and different sources of anthropogenic particles in and around the western Mediterranean Basin: North African and European urban areas, the Iberian and Italian peninsulas, most forest fires and ship emissions. As a result, the aerosol direct forcing efficiency, more dependent to absorption than the absolute forcing, has no marked gradient.

Radiative forcing from anthropogenic sulfur and organic emissions reaching the stratosphere

AbstractStratospheric aerosols cool the Earth by scattering sunlight. Although sulfuric acid dominates the stratospheric aerosol, this study finds that organic material in the lowermost stratosphere contributes 30–40% of the nonvolcanic stratospheric aerosol optical depth (sAOD). Simulations indicate that nonvolcanic sAOD has increased 77% since 1850. Stratospheric aerosol accounts for 21% of the total direct aerosol radiative forcing (which is negative) and 12% of the total aerosol optical depth (AOD) increase from organics and sulfate. There is a larger stratospheric influence on radiative forcing (i.e., 21%) relative to AOD (i.e., 12%) because an increase of tropospheric black carbon warms the planet while stratospheric aerosols (including black carbon) cool the planet. Radiative forcing from nonvolcanic stratospheric aerosol mass of anthropogenic origin, including organics, has not been widely considered as a significant influence on the climate system.

Optical and radiative properties of aerosols over Desalpar, a remote site in western India: Source identification, modification processes and aerosol type discrimination

Aerosol optical properties are analyzed for the first time over Desalpar (23.74°N, 70.69°E, 30m above mean sea level) a remote site in western India during October 2014 to August 2015. Spectral aerosol optical depth (AOD) measurements were performed using the CIMEL CE-318 automatic Sun/sky radiometer. The annual-averaged AOD500 and Ångström exponent (α440–870) values are found to be 0.43±0.26 and 0.69±0.39, respectively. On the seasonal basis, high AOD500 of 0.45±0.30 and 0.61±0.34 along with low α440–870 of 0.41±0.27 and 0.41±0.35 during spring (March–May) and summer (June–August), respectively, suggest the dominance of coarse-mode aerosols, while significant contribution from anthropogenic sources is observed in autumn (AOD500=0.47±0.26, α440–870=1.02±0.27). The volume size distribution and the spectral single-scattering albedo also confirm the presence of coarse-mode aerosols during March–August. An overall dominance of a mixed type of aerosols (~56%) mostly from October to February is found via the AOD500 vs α440–870 relationship, while marine aerosols contribute to ~18%. Spectral dependence of α and its second derivative (α′) are also used for studying the aerosol modification processes. The average direct aerosol radiative forcing (DARF) computed via the SBDART model is estimated to range from −27.08Wm−2 to −10.74Wm−2 at the top of the atmosphere, from −52.21Wm−2 to −21.71Wm−2 at the surface and from 10.97Wm−2 to 26.54Wm−2 within the atmosphere. This atmospheric forcing translates into heating rates of 0.31–0.75Kday−1. The aerosol properties and DARF are also examined for different trajectory clusters in order to identify the sources and to assess the influence of long-range transported aerosols over Desalpar.

Global climate forcing of aerosols embodied in international trade

International trade separates regions consuming goods and services from regions where goods and related aerosol pollution are produced. Yet the role of trade in aerosol climate forcing attributed to different regions has never been quantified. Here, we contrast the direct radiative forcing of aerosols related to regions’ consumption of goods and services against the forcing due to emissions produced in each region. Aerosols assessed include black carbon, primary organic aerosol, and secondary inorganic aerosols, including sulfate, nitrate and ammonium. We find that global aerosol radiative forcing due to emissions produced in East Asia is much stronger than the forcing related to goods and services ultimately consumed in that region because of its large net export of emissions-intensive goods. The opposite is true for net importers such as Western Europe and North America: global radiative forcing related to consumption is much greater than the forcing due to emissions produced in these regions. Overall, trade is associated with a shift of radiative forcing from net importing to net exporting regions. Compared to greenhouse gases such as carbon dioxide, the short atmospheric lifetimes of aerosols cause large localized differences between consumption- and production-related radiative forcing. International efforts to reduce emissions in the exporting countries will help alleviate trade-related climate and health impacts of aerosols while lowering global emissions.

Tethered balloon-born and ground-based measurements of black carbon and particulate profiles within the lower troposphere during the foggy period in Delhi, India

The ground and vertical profiles of particulate matter (PM) were mapped as part of a pilot study using a Tethered balloon within the lower troposphere (1000m) during the foggy episodes in the winter season of 2015–16 in New Delhi, India. Measurements of black carbon (BC) aerosol and PM <2.5 and 10μm (PM2.5 & PM10 respectively) concentrations and their associated particulate optical properties along with meteorological parameters were made. The mean concentrations of PM2.5, PM10, BC370nm, and BC880nm were observed to be 146.8±42.1, 245.4±65.4, 30.3±12.2, and 24.1±10.3μgm−3, respectively. The mean value of PM2.5 was ~12 times higher than the annual US-EPA air quality standard. The fraction of BC in PM2.5 that contributed to absorption in the shorter visible wavelengths (BC370nm) was ~21%. Compared to clear days, the ground level mass concentrations of PM2.5 and BC370nm particles were substantially increased (59% and 24%, respectively) during the foggy episode. The aerosol light extinction coefficient (σext) value was much higher (mean: 610Mm−1) during the lower visibility (foggy) condition. Higher concentrations of PM2.5 (89μgm−3) and longer visible wavelength absorbing BC880nm (25.7μgm−3) particles were observed up to 200m. The BC880nm and PM2.5 aerosol concentrations near boundary layer (1km) were significantly higher (~1.9 and 12μgm−3), respectively. The BC (i.e BCtot) aerosol direct radiative forcing (DRF) values were estimated at the top of the atmosphere (TOA), surface (SFC), and atmosphere (ATM) and its resultant forcing were - 75.5Wm−2 at SFC indicating the cooling effect at the surface. A positive value (20.9Wm−2) of BC aerosol DRF at TOA indicated the warming effect at the top of the atmosphere over the study region. The net DRF value due to BC aerosol was positive (96.4Wm−2) indicating a net warming effect in the atmosphere. The contribution of fossil and biomass fuels to the observed BC aerosol DRF values was ~78% and ~22%, respectively. The higher mean atmospheric heating rate (2.71Kday−1) by BC aerosol in the winter season would probably strengthen the temperature inversion leading to poor dispersion and affecting the formation of clouds. Serious detrimental impacts on regional climate due to the high concentrations of BC and PM (especially PM2.5) aerosol are likely based on this study and suggest the need for immediate, stringent measures to improve the regional air quality in the northern India.

Influence of atmospheric relative humidity on ultraviolet flux and aerosol direct radiative forcing: Observation and simulation

The atmospheric aerosols can absorb moisture from the environment due to their hydrophilicity and thus affect atmospheric radiation fluxes. In this article, the ultraviolet radiation and relative humidity (RH) data from ground observations and a radiative transfer model were used to examine the influence of RH on ultraviolet radiation flux and aerosol direct radiative forcing under the clear-sky conditions. The results show that RH has a significant influence on ultraviolet radiation because of aerosol hygroscopicity. The relationship between attenuation rate and RH can be fitted logarithmically and all of the R2 of the 4 sets of samples are high, i.e. 0.87, 0.96, 0.9, and 0.9, respectively. When the RH is 60%, 70%, 80% and 90%, the mean aerosol direct radiative forcing in ultraviolet is −4.22W m−2, −4.5W m−2, −4.82W m−2 and −5.4W m−2, respectively. For the selected polluted air samples the growth factor for computing aerosol direct radiative forcing in the ultraviolet for the RH of 80% varies from 1.19 to 1.53, with an average of 1.31.

Effects of Aerosols on Radiative Forcing and Climate Over East Asia With Different SO2 Emissions

It is known that aerosol and precursor gas emissions over East Asia may be underestimated by 50% due to the absence of data on regional rural and township industries. As the most important element of anthropogenic emissions, sulphur dioxide (SO 2 ) can form sulfate aerosols through several chemical processes, thus affecting the regional and global climate. In this study, we use the Community Atmospheric Model 5.1 (CAM5.1) to investigate the effects of anthropogenic aerosols on radiative forcing and the climate over East Asia, taking into consideration various SO 2 emission levels, including double the amount of SO 2 emissions over East Asia. Numerical experiments are performed using high-resolution CAM5.1 with pre-industrial (PI) and present day (PD) aerosol emission levels, and with PD aerosol emission levels with double SO 2 emissions over East Asia (PD2SO2). The simulated aerosol optical depth and surface sulfate concentrations over East Asia are significantly increased in PD2SO2, which is in better agreement with the observational results. The simulation results show extensive aerosol direct and indirect radiative forcing for PD−PI (the difference between PI and PD), which significantly weakens the large-scale intensity of the East Asian summer monsoon (EASM) and reduces the summer precipitation. Compared to PD, the aerosol direct radiative forcing is significantly increased in PD2SO2, whereas the aerosol indirect radiative forcing is markedly decreased due to the inhibition of cloud formation, especially over North China. The increase in aerosol direct radiative forcing and decrease in aerosol indirect radiative forcing result in insignificant changes in the total amount of aerosol radiative forcing. These results also show that the large-scale intensity of the EASM and the associated summer precipitation are insensitive to the doubling of current SO 2 emissions.

Global fine-mode aerosol radiative effect, as constrained by comprehensive observations

Abstract. Aerosols directly affect the radiative balance of the Earth through the absorption and scattering of solar radiation. Although the contributions of absorption (heating) and scattering (cooling) of sunlight have proved difficult to quantify, the consensus is that anthropogenic aerosols cool the climate, partially offsetting the warming by rising greenhouse gas concentrations. Recent estimates of global direct anthropogenic aerosol radiative forcing (i.e., global radiative forcing due to aerosol–radiation interactions) are −0.35 ± 0.5 W m−2, and these estimates depend heavily on aerosol simulation. Here, we integrate a comprehensive suite of satellite and ground-based observations to constrain total aerosol optical depth (AOD), its fine-mode fraction, the vertical distribution of aerosols and clouds, and the collocation of clouds and overlying aerosols. We find that the direct fine-mode aerosol radiative effect is −0.46 W m−2 (−0.54 to −0.39 W m−2). Fine-mode aerosols include sea salt and dust aerosols, and we find that these natural aerosols result in a very large cooling (−0.44 to −0.26 W m−2) when constrained by observations. When the contribution of these natural aerosols is subtracted from the fine-mode radiative effect, the net becomes −0.11 (−0.28 to +0.05) W m−2. This net arises from total (natural + anthropogenic) carbonaceous, sulfate and nitrate aerosols, which suggests that global direct anthropogenic aerosol radiative forcing is less negative than −0.35 W m−2.

On the influence of the diurnal variations of aerosol content to estimate direct aerosol radiative forcing using MODIS data

Long-term measurements of aerosol optical depth (AOD) from the Aerosol Robotic Network (AERONET) located in Beijing reveal a strong diurnal cycle of aerosol load staged by seasonal patterns. Such pronounced variability is matter of importance in respect to the estimation of daily averaged direct aerosol radiative forcing (DARF). Polar-orbiting satellites could only offer a daily revisit, which turns in fact to be even much less in case of frequent cloudiness. Indeed, this places a severe limit to properly capture the diurnal variations of AOD and thus estimate daily DARF. Bearing this in mind, the objective of the present study is however to evaluate the impact of AOD diurnal variations for conducting quantitative assessment of DARF using Moderate Resolution Imaging Spectroradiometer (MODIS) AOD data over Beijing. We provide assessments of DARF with two different assumptions about diurnal AOD variability: taking the observed hourly-averaged AOD cycle into account and assuming constant MODIS (including Terra and Aqua) AOD value throughout the daytime. Due to the AOD diurnal variability, the absolute differences in annual daily mean DARFs, if the constant MODIS/Terra (MODIS/Aqua) AOD value is used instead of accounting for the observed hourly-averaged daily variability, is 1.2 (1.3) Wm−2 at the top of the atmosphere, 27.5 (30.6) Wm−2 at the surface, and 26.4 (29.3) Wm−2 in the atmosphere, respectively. During the summertime, the impact of the diurnal AOD variability on seasonal daily mean DARF estimates using MODIS Terra (Aqua) data can reach up to 2.2 (3.9) Wm−2 at the top of the atmosphere, 43.7 (72.7) Wm−2 at the surface, and 41.4 (68.8) Wm−2 in the atmosphere, respectively. Overall, the diurnal variation in AOD tends to cause large bias in the estimated DARF on both seasonal and annual scales. In summertime, the higher the surface albedo, the stronger impact on DARF at the top of the atmosphere caused by dust and biomass burning (continental) aerosol. This indicates that the impact on DARFs estimates is sensitive to assumptions of aerosol type and surface albedo.

Direct radiative forcing properties of atmospheric aerosols over semi-arid region, Anantapur in India

This paper describes the aerosols optical, physical characteristics and the aerosol radiative forcing pertaining to semi-arid region, Anantapur for the period January 2013-December 2014. Collocated measurements of Aerosol Optical Depth (AOD) and Black Carbon mass concentration (BC) are carried out by using MICROTOPS II and Aethalometer and estimated the aerosol radiative forcing over this location. The mean values of AOD at 500nm are found to be 0.47±0.09, 0.34±0.08, 0.29±0.06 and 0.30±0.07 during summer, winter, monsoon and post-monsoon respectively. The Angstrom exponent (α380–1020) value is observed maximum in March (1.25±0.19) and which indicates the predominance of fine - mode aerosols and lowest in the month of July (0.33±0.14) and may be due to the dominance of coarse-mode aerosols.The diurnal variation of BC is exhibited two height peaks during morning 07:00–08:00 (IST) and evening 19:00–21:00 (IST) hours and one minima noticed during afternoon (13:00–16:00). The highest monthly mean BC concentration is observed in the month of January (3.4±1.2μgm−3) and the lowest in July (1.1±0.2μgm−3).The estimated Aerosol Direct Radiative Forcing (ADRF) in the atmosphere is found to be +36.8±1.7Wm−2, +26.9±0.2Wm−2, +18.0±0.6Wm−2 and +18.5±3.1Wm−2 during summer, winter, monsoon and post-monsoon seasons, respectively. Large difference between TOA and BOA forcing is observed during summer which indicate the large absorption of radiant energy (36.80Wm−2) which contributes more increase in atmospheric heating by ~1K/day. The BC contribution on an average is found to be 64% and is responsible for aerosol atmospheric heating.

Synergistic use of Lagrangian dispersion and radiative transfer modelling with satellite and surface remote sensing measurements for the investigation of volcanic plumes: the Mount Etna eruption of 25–27 October 2013

Abstract. In this paper we combine SO2 and ash plume dispersion modelling with satellite and surface remote sensing observations to study the regional influence of a relatively weak volcanic eruption from Mount Etna on the optical and micro-physical properties of Mediterranean aerosols. We analyse the Mount Etna eruption episode of 25–27 October 2013. The evolution of the plume along the trajectory is investigated by means of the FLEXible PARTicle Lagrangian dispersion (FLEXPART) model. The satellite data set includes true colour images, retrieved values of volcanic SO2 and ash, estimates of SO2 and ash emission rates derived from MODIS (MODerate resolution Imaging Spectroradiometer) observations and estimates of cloud top pressure from SEVIRI (Spinning Enhanced Visible and InfraRed Imager). Surface remote sensing measurements of aerosol and SO2 made at the ENEA Station for Climate Observations (35.52° N, 12.63° E; 50 m a.s.l.) on the island of Lampedusa are used in the analysis. The combination of these different data sets suggests that SO2 and ash, despite the initial injection at about 7.0 km altitude, reached altitudes around 10–12 km and influenced the column average aerosol particle size distribution at a distance of more than 350 km downwind. This study indicates that even a relatively weak volcanic eruption may produce an observable effect on the aerosol properties at the regional scale. The impact of secondary sulfate particles on the aerosol size distribution at Lampedusa is discussed and estimates of the clear-sky direct aerosol radiative forcing are derived. Daily shortwave radiative forcing efficiencies, i.e. radiative forcing per unit AOD (aerosol optical depth), are calculated with the LibRadtran model. They are estimated between −39 and −48 W m−2 AOD−1 at the top of the atmosphere and between −66 and −49 W m−2 AOD−1 at the surface, with the variability in the estimates mainly depending on the aerosol single scattering albedo. These results suggest that sulfate particles played a large role in the transported plume composition and radiative forcing, while the contribution by ash particles was small in the volcanic plume arriving at Lampedusa during this event.

Column-integrated aerosol optical properties and direct radiative forcing over the urban-industrial megacity Nanjing in the Yangtze River Delta, China.

Aerosol optical properties were measured and analyzed through the ground-based remote sensing Aerosol Robotic Network (AERONET) over an urban-industrial site, Nanjing (32.21° N, 118.72° E, and 62m above sea level), in the Yangtze River Delta, China, during September 2007-August 2008. The annual averaged values of aerosol optical depth (AOD500) and the Ångström exponent (AE440-870) were measured to be 0.94 ± 0.52 and 1.10 ± 0.21, respectively. The seasonal averaged values of AOD500 (AE440-870) were noticed to be high in summer (autumn) and low in autumn (spring). The characterization of aerosol types showed the dominance of mixed type followed by the biomass burning and urban-industrial type of aerosol at Nanjing. Subsequently, the curvature (a 2) obtained from the second-order polynomial fit and the second derivative of AE (α') were also analyzed to understand the dominant aerosol type. The single scattering albedo at 440nm (SSA440) varied from 0.88 to 0.93 with relatively lower (higher) values during the summer (spring), suggesting an increase in black carbon and mineral dust (desert dust) aerosols of absorbing (scattering) nature. The averaged monthly and seasonal evolutions of shortwave (0.3-4.0μm) direct aerosol radiative forcing (DARF) values were computed from the Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART) model both at the top of atmosphere (TOA) and bottom of atmosphere (SUR) during the study period. Further, the aerosol forcing efficiency (AFE) and the corresponding atmospheric heating rates (AHR) were also estimated from the forcing within the atmosphere (ATM). The derived DARF values, therefore, produced a warming effect within the atmosphere due to strong absorption of solar radiation.

Influence of the vertical absorption profile of mixed Asian dust plumes on aerosol direct radiative forcing over East Asia

We estimate the aerosol direct radiative forcing (ADRF) and heating rate profiles of mixed East Asian dust plumes in the solar wavelength region ranging from 0.25 to 4.0 μm using the Santa Barbara Discrete Ordinate Atmospheric Radiative Transfer (SBDART) code. Vertical profiles of aerosol extinction coefficients and single-scattering albedos (SSA) were derived from measurements with a multi-wavelength Raman lidar system. The data are used as input parameters for our radiative transfer calculations. We considered four cases of radiative forcing in SBDART: 1. dust, 2. pollution, 3. mixed dust plume and the use of vertical profiles of SSA, and 4. mixed dust plumes and the use of column-averaged values of SSA. In our sensitivity study we examined the influence of SSA and aerosol layer height on our results. The ADRF at the surface and in the atmosphere shows a small dependence on the specific shape of the aerosol extinction vertical profile and its light-absorption property for all four cases. In contrast, at the top of the atmosphere (TOA), the ADRF is largely affected by the vertical distribution of the aerosols extinction. This effect increases if the light-absorption capacity (decrease of SSA) of the aerosols increases. We find different radiative effects in situations in which two layers of aerosols had different light-absorption properties. The largest difference was observed at the TOA for an absorbing aerosol layer at high altitude in which we considered in one case the vertical profile of SSA and in another case the column-averaged SSA only. The ADRF at the TOA increases when the light-absorbing aerosol layer is located above 3 km altitude. The differences between height-resolved SSA, which can be obtained from lidar data, and total layer-mean SSA indicates that the use of a layer-mean SSA can be rather misleading as it can induce a large error in the calculation of the ADRF at the TOA, which in turn may cause errors in the vertical profiles of heating rates.

Quantifying enhancement in aerosol radiative forcing during ‘extreme aerosol days’ in summer at Delhi National Capital Region, India

Changes in aerosol characteristics (spectral aerosol optical depth, AOD and composition) are examined during the transition from ‘relatively clean’ to ‘extreme’ aerosol days in the summer of 2012 at Delhi National Capital Region (NCR), India. AOD smaller than 0.54 (i.e. 12-year mean AOD−1σ) represents ‘relatively clean’ days in Delhi during the summer. ‘Extreme’ days are defined by the condition when AOD0.5 exceeds 12-year mean AOD+1 standard deviation (σ). Mean (±1σ) AOD increases to 1.2±0.12 along with a decrease of Angstrom Exponent from 0.54±0.09 to 0.22±0.12 during the ‘extreme’ days. Aerosol composition is inferred by fixing the number concentrations of various individual species through iterative tweaking when simulated (following Mie theory) AOD spectrum matches with the measured one. Contribution of coarse mode dust to aerosol mass increased from 76.8% (relatively clean) to 96.8% (extreme events), while the corresponding contributions to AOD0.5 increased from 35.0% to 70.8%. Spectrally increasing single scattering albedo (SSA) and CALIPSO aerosol sub-type information support the dominant presence of dust during the ‘extreme’ aerosol days. Aerosol direct radiative forcing (ADRF) at the top-of-the-atmosphere increases from 21.2Wm−2 (relatively clean) to 56.6Wm−2 (extreme), while the corresponding change in surface ADRF is from −99.5Wm−2 to −153.5Wm−2. Coarse mode dust contributes 60.3% of the observed surface ADRF during the ‘extreme’ days. On the contrary, 0.4% mass fraction of black carbon (BC) translates into 13.1% contribution to AOD0.5 and 33.5% to surface ADRF during the ‘extreme’ days. The atmospheric heating rate increased by 75.1% from 1.7K/day to 2.96K/day during the ‘extreme’ days.

Overview of the Chemistry-Aerosol Mediterranean Experiment/Aerosol Direct Radiative Forcing on the Mediterranean Climate (ChArMEx/ADRIMED) summer 2013 campaign

The Chemistry-Aerosol Mediterranean Experiment (ChArMEx; http://charmex.lsce.ipsl.fr) is a collaborative research program federating international activities to investigate Mediterranean regional chemistry-climate interactions. A special observing period (SOP-1a) including intensive airborne measurements was performed in the framework of the Aerosol Direct Radiative Forcing on the Mediterranean Climate (ADRIMED) project during the Mediterranean dry season over the western and central Mediterranean basins, with a focus on aerosol-radiation measurements and their modeling. The SOP-1a took place from 11 June to 5 July 2013. Airborne measurements were made by both the ATR-42 and F-20 French research aircraft operated from Sardinia (Italy) and instrumented for in situ and remote-sensing measurements, respectively, and by sounding and drifting balloons, launched in Minorca. The experimental set-up also involved several ground-based measurement sites on islands including two ground-based reference stations in Corsica and Lampedusa and secondary monitoring sites in Minorca and Sicily. Additional measurements including lidar profiling were also performed on alert during aircraft operations at EARLINET/ACTRIS stations at Granada and Barcelona in Spain, and in southern Italy. Remote sensing aerosol products from satellites (MSG/SEVIRI, MODIS) and from the AERONET/PHOTONS network were also used. Dedicated meso-scale and regional modelling experiments were performed in relation to this observational effort. We provide here an overview of the different surface and aircraft observations deployed during the ChArMEx/ADRIMED period and of associated modeling studies together with an analysis of the synoptic conditions that determined the aerosol emission and transport. Meteorological conditions observed during this campaign (moderate temperatures and southern flows) were not favorable to produce high level of atmospheric pollutants nor intense biomass burning events in the region. However, numerous mineral dust plumes were observed during the campaign with main sources located in Morocco, Algeria and Tunisia, leading to aerosol optical depth (AOD) values ranging between 0.2 to 0.6 (at 440 nm) over the western and central Mediterranean basins. Associated aerosol extinction values measured on-board the ATR-42 within the dust plume show local maxima reaching up to 150 Mm−1. Non negligible aerosol extinction (about 50 Mm−1) was also been observed within the Marine Boundary Layer (MBL). By combining ATR-42 extinction, absorption and scattering measurements, a complete optical closure has been made revealing excellent agreement with estimated optical properties. Associated calculations of the dust single scattering albedo (SSA) have been conducted, which show a moderate variability (from 0.90 to 1.00 at 530 nm). In parallel, active remote-sensing observations from the surface and onboard the F-20 aircraft suggest a complex vertical structure of particles and distinct aerosol layers with sea-salt and pollution located within the MBL, and mineral dust and/or aged north American smoke particles located above (up to 6–7 km in altitude). Aircraft and balloon-borne observations show particle size distributions characterized by large aerosols (> 10 μm in diameter) within dust plumes. In terms of shortwave (SW) direct forcing, in-situ surface and aircraft observations have been merged and used as inputs in 1-D radiative transfer codes for calculating the direct radiative forcing (DRF). Results show significant surface SW instantaneous forcing (up to −90 W m−2 at noon). Associated 3-D modeling studies from regional climate (RCM) and chemistry transport (CTM) models indicate a relatively good agreement for simulated AOD compared with measurements/observations from the AERONET/PHOTONS network and satellite data, especially for long-range dust transport. Calculations of the 3-D SW (clear-sky) surface DRF indicate an average of about −10 to −20 W m−2 (for the whole period) over the Mediterranean Sea together with maxima (−50 W m−2) over northern Africa. The top of the atmosphere (TOA) DRF is shown to be highly variable within the domain, due to moderate absorbing properties of dust and changes in the surface albedo. Indeed, 3-D simulations indicate negative forcing over the Mediterranean Sea and Europe and positive forcing over northern Africa.